Searching alternatives to Pt-based catalyst for producing hydrogen via water splitting has gathered enormous attention to develop renewable energy. Phosphorene has been investigated widely for its large surface area, ...Searching alternatives to Pt-based catalyst for producing hydrogen via water splitting has gathered enormous attention to develop renewable energy. Phosphorene has been investigated widely for its large surface area, low cost, and high carrier mobility, however, the poor activity in hydrogen evolution reaction (HER) and low conductivity limit its practical application. Herein, on the basis of first-principles calculations, we demonstrate that the catalytic HER in phosphorene can be enhanced significantly with cobalt intercalations. The Co-intercalated phosphorene is metallic with charge transfer from Co atoms to phosphorene, which could enhance the catalytic activity of phosphorene. In addition, the calculated Gibbs free energy of hydrogen adsorption on Co-intercalated phosphorene bilayer is comparable to that on Pt(111) surface, independent of the degree of hydrogen coverage. Our study implies that the Co intercalation provides an effective approach to enhance the catalytic HER in phosphorene.展开更多
Hydrided Mg-3Ni-2MnO2 composite powders were fabricated by reactive ball milling with hydrogen, and accumulative hydrogenation kinetics and temperature field of reaction bed with various porosities (0.37, 0.53 and 0.6...Hydrided Mg-3Ni-2MnO2 composite powders were fabricated by reactive ball milling with hydrogen, and accumulative hydrogenation kinetics and temperature field of reaction bed with various porosities (0.37, 0.53 and 0.63) were measured. The results show that the accumulative hydrogenation kinetics of Mg-3Ni-2MnO2 powder reaction bed depends strongly on the effect of heat transfer, mass transfer and intrinsic reaction together. The reaction bed with the porosity of 0.53 exhibits the largest hydrogenation rate. During the hydrogenation process, the temperature of reaction bed rises quickly due to the fast release of heat, and the temperature difference between center and wall with 0.53 porosity can keep high even for a long time, which promotes fast heat transfer. The further analysis indicates that more emphases should be put on heat transfer rate rather than the only improvement of the effective thermal conductivity.展开更多
Possibilities for enhancement of catalytic reaction rate by combining phase transfer catalysis and hydrogen bonding of the catalyst with the substrate and reagent were studied. A phase transfer catalyst library with s...Possibilities for enhancement of catalytic reaction rate by combining phase transfer catalysis and hydrogen bonding of the catalyst with the substrate and reagent were studied. A phase transfer catalyst library with sixty polystyrene-supported quaternary ammonium salt catalysts was synthesized. The reduction of acetophenone by NaBH, was used as the probing reaction to select out the most active catalyst in the library by using iterative method, which was the gel-type triethanolamine aminating strongly basic anion exchange resin with the crosslinking degree of 2% A hydrogen bonding assisted catalytic mechanism was proposed to explain the high catalytic activity of the catalyst.展开更多
The asymmetric nitro-Mannich reaction is one of the traditional methods for forming carbon-carbon bond. By this reaction, the corresponding products with two contiguous stereocenters containing nitrogen substituents c...The asymmetric nitro-Mannich reaction is one of the traditional methods for forming carbon-carbon bond. By this reaction, the corresponding products with two contiguous stereocenters containing nitrogen substituents can be obtained. These β-nitro amine products can be easily transformed into 1,2-diamines by reduction of the corresponding nitro groups by means of the Nef reaction. It is well known that chiral 1,2-diamines Nay an important role in many fields.展开更多
基金the National Natural Science Foundation of China (No.21573204 and No.21421063)Ministry of Science and Technology of China (2018YFA0208603 and 2016YFA0200602)Anhui Initiative in Quantum Information Technologies, the Fundamental Research Funds for the Central UniversitiesUniversities, the National Program for Support of Top-notch Young Professional, Chinese Academy of Sciences Interdisciplinary Innovation Team, and Super Computer Center of USTC supercomputing center and CAS supercomputing center.
文摘Searching alternatives to Pt-based catalyst for producing hydrogen via water splitting has gathered enormous attention to develop renewable energy. Phosphorene has been investigated widely for its large surface area, low cost, and high carrier mobility, however, the poor activity in hydrogen evolution reaction (HER) and low conductivity limit its practical application. Herein, on the basis of first-principles calculations, we demonstrate that the catalytic HER in phosphorene can be enhanced significantly with cobalt intercalations. The Co-intercalated phosphorene is metallic with charge transfer from Co atoms to phosphorene, which could enhance the catalytic activity of phosphorene. In addition, the calculated Gibbs free energy of hydrogen adsorption on Co-intercalated phosphorene bilayer is comparable to that on Pt(111) surface, independent of the degree of hydrogen coverage. Our study implies that the Co intercalation provides an effective approach to enhance the catalytic HER in phosphorene.
基金Projects(2006126, 2006130 and 2008GG10007004) supported by the Science & Technology Plan of Shandong Province, China
文摘Hydrided Mg-3Ni-2MnO2 composite powders were fabricated by reactive ball milling with hydrogen, and accumulative hydrogenation kinetics and temperature field of reaction bed with various porosities (0.37, 0.53 and 0.63) were measured. The results show that the accumulative hydrogenation kinetics of Mg-3Ni-2MnO2 powder reaction bed depends strongly on the effect of heat transfer, mass transfer and intrinsic reaction together. The reaction bed with the porosity of 0.53 exhibits the largest hydrogenation rate. During the hydrogenation process, the temperature of reaction bed rises quickly due to the fast release of heat, and the temperature difference between center and wall with 0.53 porosity can keep high even for a long time, which promotes fast heat transfer. The further analysis indicates that more emphases should be put on heat transfer rate rather than the only improvement of the effective thermal conductivity.
基金Supported by the National Natural Science Foundation of China !(Grant No. 29574164 and 29974015)
文摘Possibilities for enhancement of catalytic reaction rate by combining phase transfer catalysis and hydrogen bonding of the catalyst with the substrate and reagent were studied. A phase transfer catalyst library with sixty polystyrene-supported quaternary ammonium salt catalysts was synthesized. The reduction of acetophenone by NaBH, was used as the probing reaction to select out the most active catalyst in the library by using iterative method, which was the gel-type triethanolamine aminating strongly basic anion exchange resin with the crosslinking degree of 2% A hydrogen bonding assisted catalytic mechanism was proposed to explain the high catalytic activity of the catalyst.
基金Supported by the National Natural Science Foundation of China（No. 51373067）.
文摘The asymmetric nitro-Mannich reaction is one of the traditional methods for forming carbon-carbon bond. By this reaction, the corresponding products with two contiguous stereocenters containing nitrogen substituents can be obtained. These β-nitro amine products can be easily transformed into 1,2-diamines by reduction of the corresponding nitro groups by means of the Nef reaction. It is well known that chiral 1,2-diamines Nay an important role in many fields.
